We report our studies of superfluorescent cascades in atomic calcium which result from two-photon excitation of several levels reasonably close to the ionization limit. We have observed significant conversion efficiencies for some of these transitions which result in subnanosecond pulses particularly in the visible wavelengths. We report the discovery of a novel two-photon scattering mechanism which could prove to be a useful method for determining collisional broadening rates. In addition, a hyper Raman transition near 17 μm is discovered which appears to be a promising candidate for a tunable source.